MOST pop acts would love to have a hit single, but be careful what you wish for. Topping the chart can be hazardous to an artist’s health, especially an out-of-nowhere hit by an unknown.

It can make a career, of course, but it can also overexpose the performer and create a backlash, set up impossible expectations and box an artist in. Just ask Beck, who spent a few years trying to shed the slacker image slapped on him by his breakthrough single “Loser.”

That was the prospect facing Gnarls Barkley when “Crazy” became a massive hit in 2006. It put the fledgling team of composer-producer Danger Mouse and singer-lyricist Cee-Lo Green on the map, collecting critical accolades and two Grammy awards. But would it throw things off balance for a partnership that was just finding its footing?

“I think if we had been a genuinely new group in our early 20s, that would have been a problem,” says Danger Mouse, who’s 30 and began making records in the late ‘90s. “We wouldn’t have had much context for what was going on.

“But I think we both had plenty of experience. . . . It was a big leap in certain ways, but it didn’t make us leap very much. We kind of stayed where we were mentally. We had each other to bounce off of.”

“Crazy’s” popularity also kept Danger Mouse and Cee-Lo on tour much longer than planned, another challenge for two musicians not especially attuned to the road life. That turned out to be a blessing in disguise.

Says Danger Mouse, “I think the intensity of being with each other for that year and change -- most people, I guess, it kind of breaks them up; for us, it got us kind of closer.”

How close? Well, for all the photos promoting their new album “The Odd Couple,” they’re dressing as bride and groom.

“Those images of the marriage and the name ‘Odd Couple’ are symbolic of our commitment to it,” says Green, sitting in a Beverly Hills hotel suite with Danger Mouse during a recent round of prerelease interviews.

“He’s the bride,” adds Danger Mouse, indicating the rotund singer sitting to his left. “You kind of could have guessed that, wouldn’t you? Yeah? Good. . . . I think most people would have guessed who would have been the one to have the [courage] to wear a dress.”

A serious side

DANGER MOUSE’S playful moment is a brief shift from the serious, analytical tone that marks most of his conversation. A music junkie (he tries to listen to a new album every day) with a taste for both indie and hip-hop, the Los Angeles-based artist, born Brian Burton, has always been a heavy thinker as well as an instinctive experimenter.

He became a critical and cultural hero in 2004 when “The Grey Album,” his unauthorized mixing of Jay-Z and Beatles recordings, demonstrated the potential of the mash-up and became a flash point in the debate over sampling and intellectual property rights.

Since then he’s carved a distinguished career as a producer, working with British musician Damon Albarn on the Gorillaz’ hit album “Demon Days” and with acclaimed cult artists such as Sparklehorse and the Black Keys. He’s currently producing Beck’s new recording.

His beautiful bride, Green, 33, was an offbeat presence on the Atlanta rap scene, working with the Goodie Mob and releasing two solo albums that established his persona as a soul/rap preacher of boundless imagination. The second, the acclaimed “Cee-Lo Green Is the Soul Machine,” was widely likened to OutKast’s “Speakerboxxx/The Love Below.”

When the two started collaborating, with Green writing lyrics and adding melodies to tracks created by Burton, the chemistry was cooking. They financed the recording of “St. Elsewhere” by themselves, then signed with the Atlantic Records-affiliated Downtown label.

The U.S. sales of 1.4 million were accompanied by critical acclaim and a widespread fascination with an enterprise that made a mission of being hard to define, from its jokey name to its eclectic music to its policy of dressing in costume -- including “Wizard of Oz” and “Star Wars” characters as well as chefs and astronauts -- on stage.

“Gnarls has really defied expectations at every step,” says Jeff Antebi, the group’s Los Angeles-based manager. “I think the industry perception was it was going to be studio-driven project, but the band did a year’s worth of worldwide touring. . . .

“And more recently, I think people assumed that Danger Mouse would go off and do one thing and Cee-Lo would go off and do another thing, but before you knew it, they have another album.

“They are both very conscious about sustaining momentum for not just themselves, but for music fans in general. They might defy expectations again, because I’m positive they are already starting to conceptualize the notion of doing another album.”

Not to get ahead of ourselves. The happy couple is still in honeymoon mode here, ready for a next step into a future they’re making up as they go along.

“We trusted each other even more,” Burton says of the making of the new album. “We had listened to a lot of music together as well, and we just kind of continued on, really. . . . We just started recording, and one of the first songs was ‘Save My Soul,’ and it sounded like a Gnarls song. ‘OK, we can still do this,’ and we kept recording.”

Reviews for “The Odd Couple,” which was rushed out in mid-March after Internet leaks torpedoed its planned April release, have been more mixed than those for “St. Elsewhere,” but Burton lines up with those who hear it as less immediately catchy but musically and emotionally deeper.

“Cee-Lo picks through that stuff I send him, and he picked the more challenging stuff. . . . And he would do things with it -- there was stuff that we did where initially I didn’t know what to think myself, and when I sat with it it made a lot more sense. I’m always experimenting, I’m always interested to see what he can possibly do with this.

“Some of his counter melodies, and even some of the changes, like how some of the changes are not as hooky as you think they are until you realize that they’re very layered. . . . He brings out stuff in the music sometimes that was almost accidental or that I didn’t think was the main part of it, and he accents that thing.”

Green doesn’t say much this afternoon, but his work on “The Odd Couple” affirms his position as pop’s operatic tenor of tormented soul. Even more than on “St. Elsewhere,” his songs explore elemental struggles, with images of being “entered by evil” and “keeping the beast at bay.”

“It’s what I know best,” he says softly. “It’s what I’m most familiar with. Wish I had other things to think about, though.” He laughs, adding, “The compositions themselves, they just reminded me of the lyrics and the life experience. It just reminds me of things I know to be true.”

The album has its lighter moments too, but one thing it doesn’t have is an obvious successor to “Crazy.”

“I think we can commend each other on genuinely not even being concerned,” Green says.

Adds Burton, “When we say we don’t care, it’s not that we’re not happy about certain things. It’s just that we know enough to not be too caught up in it. It’s fun to have a big song that people can sing. . . . When we started making this record, we loved the idea that people were going to wait to hear what we we’re going to do next. . . . I don’t know if we’re going to have any other songs like that, but we had at least one.”